FB-CVD方法制备SiC包覆层过程中的MTS裂解气体分析
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- 英文论文题名：The analysis of the pyrolysis gas of MTS during the preparation of SiC coating layer using FB-CVD method
- 论文作者：王子梁 ; 刘荣正 ; 刘马林 ; 常家兴 ; 刘兵 ; 邵友林 ; 王永欣
- 英文论文作者：WANG Zi-liang ; LIU Rong-zheng ; LIU Ma-lin ; CHANG Jia-xing ; LIU Bing ; SHAO You-lin ; WANG Yong-xin ; Institute Of Nuclear And New Energy Technology ; Tsinghua University ; Northwestern Polytechnical University
- 年：2015
- 作者机构：清华大学核能与新能源技术研究院;西北工业大学;
- 论文关键词：SiC ; MTS ; 气相色谱 ; 裂解 ; 气相分析
- 英文论文关键词：SiC ; MTS ; GC ; pyrolysis ; gas phase analysis
- 会议召开时间：2015-09-21
- 会议录名称：中国核科学技术进展报告（第四卷）——中国核学会2015年学术年会论文集第5册（核材料分卷、辐射防护分卷）
- 语种：中文
- 分类号：TL424
- 学会代码：EGVD
- 会议名称：中国核学会2015年学术年会
- 会议地点：中国四川绵阳
- 主办单位：中国核学会
- 学会名称：中国核学会
- 页数：6
- 文件大小：349k
- 原文格式：O
- 会议级别：全国
摘要
高温气冷堆核燃料元件采用TRISO型四层包覆燃料颗粒,其中SiC层是阻挡裂变产物的关键层,为采用流化床-化学气相沉积(FB-CVD)方法制备而成。进行包覆燃料颗粒SiC层前驱体的裂解过程研究,对优化SiC包覆层的制备有一定的指导意义。文献中多考虑1 300℃以下固定床中甲基三氯硅烷(MTS)裂解过程分析,对流化床和高温条件下MTS裂解制备SiC包覆层的气体分析研究较少。本文以MTS为前驱体原料,采用流化床-化学气相沉积的方法在模拟颗粒上沉积SiC层,对MTS前驱体的裂解气体进行气相色谱(GC)定性定量分析,研究温度对气相组成的影响,并反推MTS裂解反应机理。主要结论如下:流化床中高温裂解气主要以CH_4、HCl为主,且沉积温度对裂解气体组成有重要影响,并给出高温条件下MTS裂解反应的主要路径。
TRISO-coated fuel particles are used in the fuel element of high-temperature gas-cooled reactors(HTGR).The study of the pyrolysis process of precursor has certain significance on the preparation of silicon carbide coating layer.In this paper,methyltrichlorosilane(MTS) was used as the precursor,SiC layer was deposited on surrogate particles(zirconium oxide) using a fluidized bed chemical vapor deposition(FB-CVD) method.Qualitative and quantitative analyses of the pyrolysis gases were carried out to investigate the effect of the deposition temperature on the composition of the gas phase through GC method.The main conclusions are obtained as follows:Pyrolysis gases mainly contain CH_4 and HCl,and the deposition temperature has a significant impact on the composition of pyrolysis gases.Also,the main route of MTS pyrolysis at high temperature in fluidized bed is recommended.
TRISO-coated fuel particles are used in the fuel element of high-temperature gas-cooled reactors(HTGR).The study of the pyrolysis process of precursor has certain significance on the preparation of silicon carbide coating layer.In this paper,methyltrichlorosilane(MTS) was used as the precursor,SiC layer was deposited on surrogate particles(zirconium oxide) using a fluidized bed chemical vapor deposition(FB-CVD) method.Qualitative and quantitative analyses of the pyrolysis gases were carried out to investigate the effect of the deposition temperature on the composition of the gas phase through GC method.The main conclusions are obtained as follows:Pyrolysis gases mainly contain CH_4 and HCl,and the deposition temperature has a significant impact on the composition of pyrolysis gases.Also,the main route of MTS pyrolysis at high temperature in fluidized bed is recommended.
引文
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[2]Miller G K,Petti D A,Varacalle D J,et al.Statistical approach and benchmarking for modeling of multidimensional behavior in TRISO-coated fuel particles[J].Journal of Nuclear Materials,2003,317(1):69-82.
[3]Petti D A,Buongiorno J,Maki J T,et al.Key differences in the fabrication,irradiation and high temperature accident testing of US and German TRISO-coated particle fuel,and their implications on fuel performance[J].Nuclear Engineering and Design,2003,222(2):281-297.
[4]Allendorf M D,Melius C F.Theoretical study of thermochemistry of molecules in the silicon-carbon-chlorinehydrogn system[J].The Journal of Physical Chemistry,1993,97(3):720-728.
[5]Deng J,Su K,Wang X,et al.Thermodynamics of the gas-phase reactions in chemical vapor deposition of silicon carbide with methyltrichlorosilane precursor[J].Theoretical Chemistry Accounts,2009,122(1-2):1-22.
[6]Ge Y,Gordon M S,Battaglia F,et al.Theoretical study of the pyrolysis of methyltrichlorosilane in the gas phase.1.Thermodynamics[J].The Journal of Physical Chemistry A,2007,111(8):1462-1474.
[7]Zhang W G,Huttinger K J.CVD of SiC from methyltrichlorosilane.PartⅡ:Composition of the gas phase and the deposit[J].Chemical Vapor Deposition,2001,7(4):173-181.
[8]Chollon G,Langlais F,Placide M,et al.Transient stages during the chemical vapour deposition of silicon carbide from CH_3SiCl_3/H_2:impact on the physicochemical and interfacial properties of the coatings[J].Thin Solid Films,2012,520(19):6075-6087.
[9]卢翠英,成来飞,张立同,等.化学气相沉积碳化硅的热力学分析[J].无机材料学报,2008,23(6):1189-1192.
[10]Wang X,Su K,Deng J,et al.Initial decomposition of methyltrichlorosilane in the chemical vapor deposition of silicon-carbide[J].Computational and Theoretical Chemistry,2011,967(2):265-272.
[11]Osterheld T H,Allendorf M D,Melius C F.Unimolecular decomposition of methyltrichlorosilane!RRKM calculations[J].The Journal of Physical Chemistry,1994,98(28):6995-7003.
[12]Langlais F,Loumagne F,Naslain R.Reactional mechanisms of the chemical vapour deposition of SiC-based ceramics from CH_3SiCl_3/H_2 gas precursor[J].Journal of Crystal Growth,1995,155(3):205-213.